Injection-moulded article

ABSTRACT

The present invention relates to an injection-molded item with HDT-B temperature of from 80 to 105° C. in accordance with DIN EN ISO 75-2:2004-09, comprising:
     i) from 47 to 59% by weight, based on the total weight of components i to iv, of a biodegradable aliphatic polyester;   ii) from 3 to 14% by weight, based on the total weight of components i to iv, of an aliphatic-aromatic polyester;   iii) from 15 to 24% by weight, based on the total weight of components i to iv, of polylactic acid;   iv) from 10 to 35% by weight, based on the total weight of components i to iv, of at least one mineral filler;
 
where the following applies to the compounded material comprising components i to iv: the ratio of component i to component iii in the compounded material is from 2.2 to 3.2, and the MVR of the compounded material is from 8 to 50 cm 3 /10 min in accordance with DIN EN 1133-1 of March 1, 2012 (190° C., 2.16 kg).

The present invention relates to an injection-molded item with HDT-Btemperature of from 80 to 105° C. in accordance with DIN EN ISO75-2:2004-09, comprising:

-   i) from 47 to 59% by weight, based on the total weight of components    i to iv, of a biodegradable polyester comprising;    -   i-a) from 90 to 100 mol %, based on components i-a to i-b, of        succinic acid;    -   i-b) from 0 to 10 mol %, based on components i-a to i-b, of one        or more C6-C20 dicarboxylic acids;    -   i-c) from 98 to 102 mol %, based on components i-a to i-b, of        1,3-propanediol or 1,4-butanediol;    -   i-d) from 0 to 1% by weight, based on components i-a to i-c, of        a chain extender or branching agent;-   ii) from 3 to 14% by weight, based on the total weight of components    i to iv, of an aliphatic-aromatic polyester comprising:    -   ii-a) from 30 to 70 mol %, based on components ii-a to ii-b, of        a C6-C18 dicarboxylic acid;    -   ii-b) from 30 to 70 mol %, based on components ii-a to ii-b, of        terephthalic acid;    -   ii-c) from 98 to 100 mol %, based on components ii-a to ii-b, of        1,3-propanediol or 1,4-butanediol;    -   ii-d) from 0 to 1% by weight, based on components ii-a to ii-c,        of a chain extender or branching agent;-   iii) from 15 to 24% by weight, based on the total weight of    components i to iv, of polylactic acid;-   iv) from 10 to 35% by weight, based on the total weight of    components i to iv, of at least one mineral filler;

where the following applies to the compounded material comprisingcomponents i to iv: the ratio of component i to component iii in thecompounded material is from 2.2 to 3.2, and the MVR of the compoundedmaterial is from 8 to 50 cm³/10 min in accordance with DIN EN 1133-1 ofMar. 1, 2012 (190° C., 2.16 kg).

Heat-resistant items of this type are suitable for the production ofcoffee capsules, lids for hot drinks, cutlery, containers for hotcontents, and microwave tableware.

U.S. Pat. No. 6,573,340 and WO 2005/063881 disclose filled biodegradablepolymer mixtures which comprise a soft polymer, for example analiphatic-aromatic polyester (PBAT) and a rigid polymer such aspolylactic acid (PLA). WO 2013/000847 moreover discloses filled polymermixtures made of polybutylene succinate (PBS) and PLA, and EP 1561785discloses filled polymer mixtures made of PBAT, PBS, and PLA. Althoughthe polymer mixtures disclosed in the last two documents are suitablefor injection molding, they are not suitable for applications such ascoffee capsules, lids for hot drinks, or microwave tableware, becausethey have limited heat resistance and only moderate impact resistance.

It was therefore an object of the present invention to provideinjection-molded items which do not have the abovementioneddisadvantages. A particular objective was to provide a plastic with heatresistance adequate for applications in the field of hot food and drink.A further intention was that the items have sufficiently high impactresistance to comply with the mechanical requirements applicablethereto.

Surprisingly, this property profile is possessed by an injection-moldeditem comprising:

-   from 47 to 59% by weight, preferably from 48 to 55% by weight, based    on the total weight of components i to iv, of a biodegradable    polyester comprising:    -   i-a) from 90 to 100 mol %, based on components i-a to i-b, of        succinic acid;    -   i-b) from 0 to 10 mol %, based on components i-a to i-b, of one        or more C6-C20 dicarboxylic acids;    -   i-c) from 98 to 102 mol %, based on components i-a to i-b, of        1,3-propanediol or 1,4-butanediol;    -   i-d) from 0 to 1% by weight, based on components i-a to i-c, of        a chain extender or branching agent;-   ii) from 3 to 14% by weight, preferably from 5 to 11% by weight,    based on the total weight of components i to iv, of an    aliphatic-aromatic polyester comprising:    -   ii-a) from 30 to 70 mol %, based on components ii-a to ii-b, of        a C6-C18 dicarboxylic acid;    -   ii-b) from 30 to 70 mol %, based on components ii-a to ii-b, of        terephthalic acid;    -   ii-c) from 98 to 100 mol %, based on components ii-a to ii-b, of        1,3-propanediol or 1,4-butanediol;    -   ii-d) from 0 to 1% by weight, based on components ii-a to ii-c,        of a chain extender or branching agent;-   iii) from 15 to 24% by weight, preferably from 15 to 20% by weight,    based on the total weight of components i to iv, of polylactic acid;-   from 10 to 35% by weight, preferably from 18 to 30% by weight, based    on the total weight of components i to iv, of at least one mineral    filler;

where the following applies to the compounded material comprisingcomponents i to iv: the ratio of component i to component iii in thecompounded material is from 2.2 to 3.2, and the MVR of the compoundedmaterial is from 8 to 50 cm³/10 min and preferably from 14 to 40 cm³⁶/10min in accordance with DIN EN 1133-1 of Mar. 1, 2012 (190° C., 2.16 kg).The HDT-B temperature of the items produced from these compoundedmaterials is moreover from 80 to 105° C., preferably from 85 to 100° C.,in accordance with DIN EN ISO 75-2:2004-09, and at the same time theCharpy impact resistance of these items is preferably more than 80kJ/m², in particular from 90 to 250 kJ/m², in accordance with DIN EN179-1/1eU:2000+Amd.A (Non-instrumented impact resistance test of Jun. 1,2001 at 23° C., 50% relative humidity).

The invention is described in more detail below.

The aliphatic polyesters i suitable for the invention are described inmore detail in

WO 2010/034711, which is expressly incorporated herein by way ofreference.

The structure of polyesters i is generally as follows:

i-a) from 90 to 100 mol %, based on components i-a to i-b, of succinicacid;

i-b) from 0 to 10 mol %, based on components i-a to i-b, of one or moreC6-C20 dicarboxylic acids;

i-c) from 98 to 102 mol %, based on components i-a to i-b, of1,3-propanediol or 1,4-butanediol;

i-d) from 0 to 1% by weight, based on components i-a to i-c, of a chainextender or branching agent.

The polyesters i described are preferably synthesized in a directpolycondensation reaction of the individual components. The dicarboxylicacid derivatives here are reacted together with the diol in the presenceof a transesterification catalyst directly to give thehigh-molecular-weight polycondensate. On the other hand, it is alsopossible to obtain the copolyester i via transesterification ofpolybutylene succinate (PBS) with C6-C20 dicarboxylic acids in thepresence of diol, Catalysts usually used are zinc catalysts, aluminumcatalysts, and in particular titanium catalysts. An advantage oftitanium catalysts such as tetra(isopropyl) orthotitanate and inparticular tetraisobutoxy titanate (TROT) over the tin catalysts,antimony catalysts, cobalt catalysts, and lead catalysts often used inthe literature, for example tin dioctanoate, is that any residualquantities of the catalyst or downstream product from the catalyst thatremain within the product are less toxic. This is a particularlyimportant factor in biodegradable polyesters because they pass directlyinto the environment.

The succinic acid, or a mixture of the dicarboxylic acids, is generallyfirst heated to an internal temperature of from 170 to 230° C. over aperiod of about 60-180 min in the presence of an excess of diol,together with the catalyst, resultant water being removed bydistillation. The melt of the prepolyester thus obtained is usuallycondensed at an internal temperature of from 200 to 250° C. within aperiod of from 3 to 6 hours at reduced pressure, while the diolliberated is removed by distillation, until the desired viscosity isreached at intrinsic viscosity (IV) of from 100 to 450 mL/g, andpreferably from 120 to 250 mL/g.

The polyesters i of the invention can moreover be produced by theprocesses described in JP 2008-45117 and EP-A 488 617. It has provenadvantageous to begin by reacting components a to c to give aprepolyester with IV of from 50 to 100 mL/g, preferably from 60 to 80mL/g, and then to react this with a chain extender i-d, for example withdiisocyanates, or with epoxy-containing polymethacrylates, in a chainextension reaction to give a polyester i with IV of from 100 to 450mL/g, preferably from 150 to 300 mL/g.

Acid component i-a used comprises from 90 to 100 mol %, based on acidcomponents a and b, preferably from 91 to 99 mol %, and with particularpreference from 92 to 98 mol %, of succinic acid. Succinic acid isaccessible by a petrochemical route, or else preferably from renewableraw materials, for example as described in EPA 2185682. EPA 2185682discloses a biotechnology process for the production of succinic acidand 1,4-butanediol starting from different carbohydrates, usingmicroorganisms from the Pasteurellaceae class.

The quantity used of acid component i-b, based on acid components i-aand i-b, is from 0 to 10 mol %, preferably from 1 to 9 mol %, and withparticular preference from 2 to 8 mol %.

The expression C6-C20 dicarboxylic acids b means in particular adipicacid, suberic acid, azelaic acid, sebacic acid, brassylic acid, and/orarachidonic acid. Preference is given to suberic acid, azelaic acid,sebacic acid, and/or brassylic acid. The abovementioned acids areaccessible from removal raw materials. By way of example, sebacic acidis accessible from castor oil. Polyesters of this type feature excellentbiodegradation performance [reference: Polym. Degr. Stab. 2004, 85,855-863].

The dicarboxylic acids i-a and i-b can be used either in the form offree acid or in the form of ester-forming derivatives. Particularester-forming derivatives that may be mentioned are the di-C₁- toC₆-alkyl esters, such as dimethyl-, diethyl-, di-n-propyl, diisopropyl,di-n-butyl, di-isobutyl, di-tent-butyl, di-n-pentyl-, diisopentyl ordi-n-hexyl esters. It is likewise possible to use anhydrides of thedicarboxylic acids. The dicarboxylic acids or ester-forming derivativesthereof can be used here individually or in the form of a mixture.

The diols 1,3-propanediol and 1,4-butanediol are likewise accessiblefrom renewable raw materials. It is also possible to use mixtures of thediols. 1,4-Butanediol is preferred as diol because the melting points ofthe resultant copolymer are higher and said copolymer exhibits bettercrystallization.

The ratio of the diol (component i-c) to the acids (components i-a andi-b) established at the start of the polymerization reaction isgenerally from 1.0:1 to 2.5:1 and preferably from 1.3:1 to 2.2:1(diol:diacids). Excess quantities of diol are drawn off during thepolymerization reaction, and the ratio obtained at the end of thepolymerization reaction is therefore approximately equimolar. Theexpression approximately equimolar means that the diacid/diol ratio isfrom 0.98 to 1,00.

One embodiment uses from 0 to 1% by weight, preferably from 0.1 to 0.9%by weight, and with particular preference from 0.1 to 0.8% by weight,based on the total weight of components i-a to i-b, of a branching agenti-d and/or chain extender i-d′ selected from the group consisting of: apolyfunctional isocyanate, isocyanurate, oxazoline, carboxylic anhydridesuch as maleic anhydride, epoxide (in particular an epoxy-containingpoly(meth)acrylate), an at least trihydric alcohol, and an at leasttribasic carboxylic acid. The general procedure uses no branchingagents, but only chain extenders.

Examples of suitable bifunctional chain extenders are tolylene2,4-diisocyanate, tolylene 2,6-diisocyanate, diphenylmethane2,2′-diisocyanate, diphenylmethane 2,4′-diisocyanate, diphenylmethane4,4′-diisocyanate, naphthylene 1,5-diisocyanate, or xylylenediisocyanate, hexamethylene 1,6-diisocyanate, isophorone diisocyanate,or methylenebis(4-isocyanato-cyclohexane). Particular preference isgiven to isophorone diisocyanate and in particular to hexamethylene1,6-diisocyanate.

The expression aliphatic polyesters i in particular means polyesterssuch as polybutylene succinate (PBS), polybutylene succinate-co-adipate(PBSA), polybutylene succinate-co-sebacate (PBSSe), polybutylenesuccinate-co-azelate (PBSAz), or polybutylene succinate-co-brassylate(PBSBr). The aliphatic polyesters PBS and PBSA are marketed by way ofexample by Showa Highpolymer as Blanche®, and by Mitsubishi as GSPIa®.WO 2010/034711 describes more recent developments.

The number-average molar mass (Mn) of the polyesters i is generally inthe range from 5000 to 100 000 g/mol, in particular in the range from 10000 to 75 000 g/mol, preferably in the range from 15 000 to 50 000glmol, their weight-average molar mass (Mw) being from 30 000 to 300 000g/mol, preferably from 60 000 to 200 000 g/mol, and their Mw/Mn ratiobeing from 1 to 6, preferably from 2 to 4. Intrinsic viscosity is from30 to 450 g/mL, preferably from 100 to 400 g/mL (measured ino-dichlorobenzene/phenol (ratio by weight 50/50)). Melting point is inthe range from 85 to 130° C., preferably in the range from 95 to 120° C.The MVR range is in the range of from 8 to 50 and in particular from 15to 40 cm³/10 min (190° C., 2.16 kg) in accordance with DIN EN 1133-1.

The expression aliphatic-aromatic polyesters ii means linear,chain-extended and optionally branched and chain-extended polyesters, asdescribed by way of example in WO 96/15173 to 15176, or in WO 98/12242,expressly incorporated herein by way of reference. Mixtures of differentsemiaromatic polyesters can likewise be used. More recent developmentsof interest are based on renewable raw materials (see WO 2010/034689).The expression polyesters ii in particular means products such asecoflex® (BASF SE).

Among the preferred polyesters ii are polyesters comprising, asessential components;

-   -   ii-a) from 30 to 70 mol %, preferably from 40 to 60 mol %, and        with particular preference from 50 to 60 mol %, based on        components ii-a) to ii-b), of an aliphatic dicarboxylic acid or        a mixture thereof, preferably as follows: adipic acid, azelaic        acid, sebacic acid, and brassylic acid,    -   ii-b) from 30 to 70 mol %, preferably from 40 to 60 mol %, and        with particular preference from 40 to 50 mol %, based on        components ii-a) and ii-b), of an aromatic dicarboxylic acid or        a mixture thereof, preferably as follows: terephthalic acid,    -   ii-c) from 98.5 to 100 mol %, based on components ii-a) to        ii-b), of 1,4-butanediol and 1,3-propanediol; and    -   ii-d) from 0 to 1% by weight, preferably from 0.1 to 0.2% by        weight, based on components ii-a) to ii-c), of a chain extender,        in particular of a di- or polyfunctional isocyanate, preferably        hexamethylene diisocyanate, and optionally of a branching agent,        preferably: trimethylolpropane, pentaerythritol, and in        particular glycerol.

Aliphatic diacids and the corresponding derivatives ii-a that can beused are generally those having from 6 to 20 carbon atoms, preferablyfrom 6 to 10 carbon atoms. They can be either linear or branchedcompounds. However, it is also in principle possible to use dicarboxylicacids having a larger number of carbon atoms, by way of example havingup to 30 carbon atoms.

Examples that may be mentioned are: 2-methylglutaric acid,3-methylglutaric acid, α-ketoglutaric acid, adipic acid, pimelic acid,azelaic acid, sebacic acid, brassylic acid, suberic acid, and itaconicacid. The dicarboxylic acids or ester-forming derivatives thereof can beused here individually or in the form of a mixture of two or morethereof.

It is preferable to use adipic acid, azelaic acid, sebacic acid,brassylic acid, or respective ester-forming derivatives of these, or amixture thereof. It is particularly preferable to use adipic acid orsebacic acid, or respective ester-forming derivatives of these, or amixture thereof.

Preference is in particular given to the following aliphatic-aromaticpolyesters: polybutylene adipate terephthalate (PEAT) and polybutylenesebacate terephthalate (PBSeT).

The aromatic dicarboxylic acids ii-b or ester-forming derivatives ofthese can be used individually or in the form of a mixture of two ormore thereof. It is particularly preferable to use terephthalic acid orits ester-forming derivatives such as dimethyl terephthalate.

The diols ii-c 1,4-butanediol and 1,3-propanediol—are accessible in theform of renewable raw material. Mixtures of the diols mentioned can alsobe used.

A general procedure uses from 0 to 1% by weight, preferably from 0.1 to1.0% by weight, and with particular preference from 0.1 to 0.3% byweight, based on the total weight of the polyester, of a branching agentand/or from 0.05 to 1% by weight, preferably from 0.1 to 1.0% by weight,based on the total weight of the polyester, of a chain extender (ii-d).Preferred branching agents and chain extenders (ii-d) are the same asthe branching agents and chain extenders (i-d) described in detailabove.

The number-average molar mass (Mn) of the polyesters ii is generally inthe range from 5000 to 100 000 g/mol, in particular in the range from 10000 to 75 000 g/mol, preferably in the range from 15 000 to 38 000g/mol, their weight-average molar mass (Mw) being from 30 000 to 300 000g/mol, preferably from 60 000 to 200 000 g/mol, and their Mw/Mn ratiobeing from 1 to 6, preferably from 2 to 4. Intrinsic viscosity is from50 to 450 g/mL, preferably from 80 to 250 g/mL (measured ino-dichlorobenzene/phenol (ratio by weight 50/50)). Melting point is inthe range from 85 to 150° C., preferably in the range from 95 to 140° C.

MVR (melt volume rate) is generally from 0.5 to 20 cm³/10 min,preferably from 5 to 15 cm³/10 min, in accordance with EN ISO 1133-1 DE(190° C., 2.16 kg weight). Acid numbers are generally from 0.01 to 1.2mg KOH/g, preferably from 0.01 to 1.0 mg KOH/g, and with particularpreference from 0.01 to 0.7 mg KOH/g, in accordance with DIN EN 12634.

Polylactic acid (PLA) is used as rigid component iii.

It is preferable to use polylactic acid with the following propertyprofiler

-   -   melt volume rate from 20 to 50 and in particular from 30 to 40        cm³/10 minutes (MVR for 190° C. and 2.16 kg in accordance with        ISO 1133-1 DE)    -   melting point below 240° C.    -   glass transition temperature (Tg) above 55° C.    -   water content smaller than 1000 ppm    -   residual content of monomers (lactide) smaller than 0.3%    -   molecular weight greater than 80 000 daltons.

Examples of preferred polylactic acids are NatureWorks® 6201 D, 6202 D,6251 D, 3051 D, and in particular 3251 D, and also crystallinepolylactic acids from NatureWorks.

The percentage proportion by weight used of the polylactic acid iii,based on components i and iv, is from 15 to 24%, preferably from 15 to20%. It is preferable here that the polylactic acid iii forms thedispersed phase and that the polyester i forms the continuous phase oris part of a cocontinuous phase. The heat resistance of polymer mixtureswith polyester i in the continuous phase or as part of a cocontinuousphase is higher than that of polymer mixtures in which polylactic acidiii forms the continuous phase. In order to ensure good heat resistancein the injection-molded item (HDT-B temperature from 85 to 105° C. inaccordance with DIN EN ISO 75-2:2004-09) the ratio of component i tocomponent iii in the compounded material from which the items areproduced should be from 2.2 to 3.2, and preferably from 2.5 to 3.1.

A general procedure uses from 10 to 35% by weight, in particular from 18to 30% by weight, and particularly preferably from 18 to 25% by weight,based on the total weight of components i to iv, of at least one mineralfiller iv selected from the group consisting of: chalk, graphite,gypsum, iron oxide, calcium chloride, dolomite, kaolin, silicon dioxide(quartz), sodium carbonate, titanium dioxide, silicate, wollastonite,mica, montmorillonites, talc powder, mineral fibers, and conductivecarbon black.

Particular preference is given to chalk and to talc powder as fillers.Interestingly, it has been found that addition of chalk can provide afurther improvement in the biodegradability of the items. Use of talcpowder can in turn be more effective in increasing modulus of elasticityand in improving heat resistance.

The compounded material of the invention comprising components i to ivcan moreover comprise other additives known to the person skilled in theart. Examples are the additional substances conventionally used inplastics technology, for example stabilizers; nucleating agents, such asthe mineral fillers iv already mentioned above, or else crystallinepolylactic acid; lubricants and release agents, such as stearates (inparticular calcium stearate); plasticizers, for example citric esters(in particular tributyl acetylcitrate), glycerol esters, such astriacetylglycerol, or ethylene glycol derivatives, surfactants, such aspolysorbates, palmitates, or laurates; waxes, for example erucamide,stearamide, or behenamide, beeswax or beeswax esters; antistatic agents,UV absorbers; UV stabilizers; antifogging agents, or dyes. Theconcentrations used of the additives are from 0 to 2% by weight, inparticular from 0.1 to 2% by weight, based on the compounded material ito iv of the invention. The compounded material i to iv of the inventioncan comprise from 0.1 to 10% by weight of plasticizers.

Mixtures of chalk and talc have proven to be particularly advantageous.A ratio of from 1:5 to 5:1 in the mixture, preferably from 1:3 to 3:1,and in particular from 1:2 to 1:1, has been found to be advantageous.

For the purposes of the present invention, a substance or a substancemixture complies with the “biodegradable” feature when said substance orthe substance mixture has a percentage degree of biodegradation of atleast 90% after 180 days in accordance with DIN EN 13432.

Biodegradability generally leads to decomposition of the polyester(mixtures) in an appropriate and demonstrable period of time. Thedegradation can take place by an enzymatic, hydrolytic, or oxidativeroute, and/or via exposure to electromagnetic radiation, for example UVradiation, and can mostly be brought about predominantly via exposure tomicroorganisms, such as bacteria, yeasts, fungi, and algae.Biodegradability can by way of example be quantified by mixing polyesterwith compost and storing the mixture for a particular time. By way ofexample, in accordance with DIN EN 13432 (with reference to ISO 14855),CO₂-free air is passed through ripened compost during the compostingprocess, and the compost is subjected to a defined temperature profile.Biodegradability here is defined as a percentage degree ofbiodegradation, by taking the ratio of the net quantity of CO₂ releasedfrom the specimen (after subtraction of the quantity of CO₂ released bythe compost without specimen) to the maximum quantity of CO₂ releasefrom the specimen (calculated from the carbon content of the specimen).Biodegradable polyesters or biodegradable polyester mixtures generallyexhibit clear signs of degradation after just a few days of composting,examples being fungal growth, cracking, and perforation.

Other methods for determining biodegradability are described by way ofexample in ASTM D5338 and ASTM D6400-4.

Injection molding, also called the injection-molding process, involves ashaping process that is very frequently used in plastics processing.Injection molding can also provide an extremely cost-effective method ofproducing large numbers of ready-to-use moldings. In simplified terms,the process functions as follows: the respective thermoplastic material(“molding composition”) is melted in an injection-molding machineconsisting of a heatable cylinder within which there is a rotatingscrew, and is injected into a metal mold. The mold cavity determines theshape and the surface structure of the finished component. Weights ofcomponents that can be produced nowadays are from well below one gram upto tens of kilograms.

Injection molding can provide a method of fast, cost-effectiveproduction of consumer articles with high precision. The nature of thesurface of the respective component here can be selected by thedesigners with almost no restriction. It is possible to produce a widevariety of surface structures, from smooth surfaces for opticalapplications by way of grained effects for regions having attractivehaptic properties through to engraved effects or other patterns.

For reasons of cost-effectiveness, the injection-molding process isparticularly suitable for the production of relative large numbers ofunits, for example of packaging items.

Items in widespread use are those such as chocolate-box inserts,games-box inserts, folding blister packs for a very wide variety ofsmall items displayed on adjustable racking in retail outlets, andyoghurt pots and margarine tubs. Lids for coffee cups or other cups forhot drinks are a preferred item, as also are packs intended to containhot foods or drinks.

A particularly preferred injection-molded item is the coffee capsule.The expression coffee capsule means a pack of volume capacity from 1 mlto 80 ml, preferably from 3 to 50 ml. A pulverulent material from thefood-or-drink sector, in particular coffee powder, or a mixture ofpulverulent materials from the food-or-drink sector, is charged to saidpack. The expression material from the food-or-drink sector means notonly coffee but also tea, milk, cocoa, and soup extracts. The shape ofthe pack can be rotationally symmetrical, conical, spherical, or elseangular, but preferably rotationally symmetrical and primarilycylindrical. Said pack serves firstly for the storage of the material(s)from the food-or-drink sector, and also for the preparation of a hotwater-based drink which is produced via passage of hot water (at from 60to 100° C.) in a subsequent step. When the water passes through the packit dissolves substances that provide flavor and bitterness, thus formingthe hot drink. The pack is intended to be manufactured via injectionmolding. The wall thickness used here for the flat film from which thepack(s) are produced has a thickness from 100 to 1000 μm, preferablyfrom 250 to 800 μm, and in particular from 155 to 550 μm. The item canbe composed of one, and preferably of a plurality of, layer(s). At leastone layer comprises the compounded material described in theintroduction comprising components i) to iv). Another layer of the finalmolded pack preferably forms a barrier layer. The multilayer structurecan be produced via coextrusion during the flat-film production processor else, after the flat-film production process, can be applied in theform of layer: for example via extrusion, printing, spraying, orsputtering, in principle by applying a dispersion, a coating material,or any other polymer-based or polymer-containing system, or by applyinga metallic or oxide-containing layer, but preferably by using apolymer-based or metalized layer. An example of a metalized layer thatcan be used is aluminum, and layers suitable as polymer-based layer arethose comprising polyglycolic acid (PGA), polyhydroxyalkanoates (PHA),for example poly-3-hydroxybutyrate (PHB),poly-3-hydroxybutyrate-co-3-hydroxyvalerate (PHB(V)),poly-3-hydroxybutyrate-co-3-hydroxy hexanoate (PHB(H)), orpoly-3-hydroxybutyrate-co-4-hydroxyvalerate; polyvinyl alcohol (PVOH),polyvinylidene chloride (PVDC), or ethylene-vinyl alcohol (EVOH). Thisbarrier layer is characterized by an oxygen transmission rate (OTR) offrom 0 to 1000 g/m²/d, measured on the entire film composite after packproduction in accordance with ASTM D1434, and also by a water vaportransmission rate of from 0 to 1000 g/m²/d in accordance with ASTMF1249, and also preferably at the same time by an aroma barrier.

The good oxygen barrier and, respectively, aroma barrier can also beachieved by means of overlap packaging for one or more coffee capsules.Suitable overlap packaging can be barrier-film-coated plastics films orpaper films.

Compounded materials comprising components i to iv that are suitable forthe injection-molding process are in particular those with MVR (190° C.,2.16 kg) of from 8 to 50 cm³/10 min in accordance with ISO 1133-1 ofMar. 1, 2012, with particular preference from 14 to 40 cm³/10 min.

Performance-Related Tests:

The molecular weights Mn and Mw of the semiaromatic polyesters weredetermined by means of SEC in accordance with DIN 55672-1: eluenthexafluoroisopropanol (HFIP)+0.05% by weight calcium trifluoroacetate;narrowly distributed polymethyl methacrylate standards were used forcalibration.

Intrinsic viscosities were determined in accordance with DIN 53728 part3, Jan. 3, 1985, Capillary viscosimetry. An M-II micro-Ubbelohdeviscosimeter was used. Solvent used was the mixture:phenol/o-dichlorobenzene in a ratio of 50/50 by weight.

The modulus of elasticity was determined by means of a tensile test ontensile specimens of thickness about 420 μm in accordance with ISO527-3: 2003.

Charpy impact resistance was determined in accordance with DIN EN179-1/1eU:2000+Amd.A (at 23° C., 50% rel. humidity). The test sample (80mm×10 mm×4 mm), in the form of horizontal bar supported close to itsends, is subjected to a single impact of a pendulum, the impact linebeing central between the two test sample supports, and the velocity ofbending (of the test sample) being high and nominally constant (2.9 or3.8 m/s).

HDT-B heat resistance was determined in accordance with DIN EN ISO75-2:2004-9. A standard test sample is subjected to three-point bendingunder constant load so as to produce a flexural stress (HDT/B0.45 MPa)stated in the relevant part of said international standard. Thetemperature is increased at uniform rate (120 K/h), and the temperaturevalue measured is that at which a defined standard deflection isreached, corresponding to the defined increased in flexural strain(0.2%).

1. Starting Materials

-   Polyester i:

i-1 Polybutylene succinate: GS-Pla® FZ71-PD from Mitsubishi ChemicalCorporation (MVR 22 cm³/10 min (190° C., 2.16 kg))

-   Polyester ii:

ii-1 Polybutylene adipate-co-terephthalate: ecoflex® F A1300 from BASFSE (MVR 8.5 cm³/10 min (190° C., 2.16 kg))

ii-2 Polybutylene sebacate-co-terephthalate: ecoflex® FS A1300 from BASFSE (MVR 8.5 cm³/10 min (190° C., 2.16 kg))

-   Component hi:

iii-1 Polylactic acid: (PLA) Ingeo® 3251 D from NatureWorks (MVR 35cm³/10 min (190° C., 2.16 kg))

-   Component iv:

iv-1 Talc IT extra from Mondo Minerals

2. Compounding

The compounding materials listed in Table 1 were manufactured in aCoperion MC 40 extruder. The discharge temperatures were set at 250° C.The extrudate was then pelletized under water. After production of thepellets, they were dried at 60° C.

3. Production of the Items (General Specification GS)

The compounded material is passed through a Ferromatik Millacron K65injection-molding machine with 30.00 mm screw. The injection mold was asingle- or multi-cavity mold with open hot runner. CAMPUS was used tomanufacture molds for the standards ISO 179/1eU and ISO 527-1/-2. Moldtemperature was 30° C. The injection pressure and hold pressure used forthe molds were 560 bar and, respectively, 800 bar.

TABLE 1 Items produced by GS: Com- Com- Com- parative parative parativeExample C1 2 3 C4 C5 Compounds* (amounts in percent by weight) i-1 59.856 52.5 48.9 45.2 ii-2 0 5 10 15 20 iii-1 22.2 21 19.5 18.1 16.8 iv-1 1818 18 18 18 i/iii-ratio 2.69 2.67 2.69 2.70 2.69 Items produced by GSHDT/B (° C.) 94.3 88.3 83.3 79.0 73.1 Charpy (kJ/m²) 76.2 94.5 119 150190 Mod. of elasticity 2625 2105 1827 1563 1329 (MPa) MVR (cm³/10 min)20.6 15.3 14.8 14.2 13.8 *the compounds each contained 0.3% by weight oferucamide, based on the compound

Examples 2 and 3 exhibit much-improved impact resistance as comparedwith C1, while maintaining a very high level of heat resistance (HDT/B).Larger amounts of aliphatic-aromatic polyester ii-2 (see 04 and C5) giveinjection-molded items with unsatisfactory distortion resistance(HDT/B).

The injection-molded items described by EP 2 540 779 have either lowimpact-resistance (addition of talc) or low heat resistance (addition ofchalk). Those with chalk feature a low barrier to oxygen as well.

1.-10. (canceled)
 11. An injection-molded item with HDT-B temperature offrom 79 to 105° C. in accordance with DIN EN ISO 75-2:2004-09,comprising: i) from 47 to 59% by weight, based on the total weight ofcomponents i to iv, of a biodegradable polyester comprising: i-a) from90 to 100 mol %, based on components a to b, of succinic acid; i-b) from0 to 10 mol %, based on components a to b, of one or more C₆-C₂₀dicarboxylic acids; i-c) from 98 to 102 mol %, based on components a tob, of 1,3-propanediol or 1,4-butanediol; i-d) from 0 to 1% by weight,based on components a to c, of a chain extender or branching agent; from3 to 14% by weight, based on the total weight of components i to iv, ofan aliphatic-aromatic polyester comprising: ii-a) from 30 to 70 mol %,based on components ii-a to ii-b, of a C₆-C₁₈-dicarboxylic acid; ii-b)from 30 to 70 mol %, based on components ii-a to ii-b, of terephthalicacid; ii-c) from 98 to 100 mol %, based on components ii-a to ii-b, of1,3-propanediol or 1,4-butanediol; ii-d) from 0 to 1% by weight, basedon components a to c, of a chain extender or branching agent; iii) from15 to 24% by weight, based on the total weight of components i to iv, ofpolylactic acid; from 10 to 35% by weight, based on the total weight ofcomponents i to iv, of at least one mineral filler; where the followingapplies to the compounded material comprising components i to iv: theratio of component i to component iii in the compounded material is from2.2 to 3.2, and the MVR of the compounded material is from 8 to 50cm³/10 min in accordance with DIN EN 1133-1 of Mar. 1, 2012 (190° C.,2.16 kg).
 12. The item according to claim 11, where the ratio ofcomponent i to component iii is from 2.5 to 3.1.
 13. The item accordingto claim 11, where the MVR of polyester i is from 15 to 40 cm³/10 min inaccordance with DIN EN 1133-1 of Mar. 1, 2012 (190° C., 2.16 kg). 14.The item according claim 11, where the MVR of polyester ii is from 5 to15 cm³/10 min in accordance with DIN EN 1133-1 of Mar. 1, 2012 (190° C.,2.16 kg).
 15. The item according claim 11, where the MVR of polyesteriii is from 30 to 40 cm³/10 min in accordance with DIN EN 1133-1 of Mar.1, 2012 (190° C., 2.16 kg).
 16. The item according claim 11, whichcomprises at least 20% by weight of a mineral filler iv, based on thetotal weight of components i to iv.
 17. The item according to claim 15,where the filler iv is talc powder.
 18. The item according to claim 11with Charpy impact resistance greater than 80 kJ/m² in accordance withDIN EN 179-1/1eU:2000.
 19. The item according to claim 11 with volumecapacity of from 1 to 80 ml, with oxygen transmission rate of from 0 to1000 g/m²/d in accordance with ASTM D1434, suitable for the productionof coffee capsules.
 20. A microwave tableware which comprises the itemaccording to claim
 11. 21. A lid of cup for hot drinks which comprisesthe item according to claim 11.